Molecule self-assembly of hydrangea-shaped hollow O, Cl −codoped graphite-phase carbon nitride microspheres for efficient N-(1,3-dimethyl butyl)-N’-phenyl-p-phenylenediamine quinone photodegradation and bacteria disinfection

• Published in: Journal of colloid and interface science Vol. 683; no. Pt 2; pp. 1049 - 1056
• Main Authors: Chen, Xiangyu, Wu, Jianhao, Wang, Xiaozhuo, Jia, Rongrong, Li, Lan, Wang, Yixuan, Cai, Yuxing, Chen, Zhi, Jin, Cheng-Chao, Wang, Xinquan, Qi, Peipei, Wang, Rongyan, Zhang, Nan
• Format: Journal Article
• Language: English
• Published: United States Elsevier Inc 01.04.2025
• Subjects: 6PPD-Q photodegradation; Anti-Bacterial Agents - chemistry; Anti-Bacterial Agents - pharmacology; antioxidants; Bacteria disinfection; carbon nitride; Disinfection; doxycycline; Graphite - chemistry; microparticles; Microspheres; Molecule self-assembly; Nitriles - chemistry; Nitrogen Compounds; Open porous carbon nitride microspheres; Particle Size; Phenylenediamines - chemistry; Phenylenediamines - pharmacology; photocatalysis; Photolysis; quinones; rubber; Staphylococcus aureus; Staphylococcus aureus - drug effects; surface area; Surface Properties; tetracycline; Treatment of antibiotic residues; 6PPD-Q photodegradation; Treatment of antibiotic residues; Open porous carbon nitride microspheres; Bacteria disinfection; Molecule self-assembly
• ISSN: 0021-9797; 1095-7103; 1095-7103
• DOI: 10.1016/j.jcis.2025.01.003

This work focused on the template-free synthesis of uniform hydrangea-shaped hollow carbon nitride microspheres (HHCN) in an intermolecular assembly process, featuring open pores with application in efficient photodegradation of 6PPD-Q, an emerging pollutant for the first time. The prepared HHCN also shows prominent performance for treating the refractory pollutants such as staphylococcus aureus and antibiotic residues. [Display omitted] •Ordered hydrangea-shaped hollow g-C3N4 microsphere was prepared by template-free ultrasound-assisted intermolecular assembly.•Unique structure and O, Cl co-doping optimize light harvesting and charge separation.•90 % of 6PPD-Q was efficiently degraded on HHCN within 60 min for the first time.•Enhanced photocatalytic activities on bacteria disinfection and antibiotic degradation are observed.•DFT calculation is used to uncover band structure and reaction mechanism. 6PPD-quinone (6PPD-Q) as a derivative of the rubber antioxidant N-(1,3-dimethylbutyl)-N’-phenyl-p-phenylenediamine (6PPD), is attracting intensive attention due to the significant hazard to ecosystems. However, the effective management of this type of contaminant has been scarcely reported. Hydrangea-like hollow O, Cl-codoped graphite-phase carbon nitride microspheres (HHCN), featuring open pores were readily prepared by molecular self-assembly and utilized to address 6PPD-Q in an aqueous system for the first time. More than 90 % of 6PPD-Q is efficiently photodegraded within 1 h on the as-prepared HHCN, which is 2.5 times more than that on bulk g-C3N4. Moreover, the as-synthesized HHCN demonstrates prominent photocatalytic activities for the degradation of doxycycline and tetracycline and the inactivation of Staphylococcus aureus (S. aureus) in an aqueous environment. The distinct hydrangea-like hollow structure imparts a large surface area and an abundance of active sites. In addition, the inclusion of Cl-3p orbitals also contributes to a reduction in the bandgap (2.01 eV) and facilitates carrier separation and transport. These combined characteristics synergistically enhance the remarkable photocatalytic performance of HHCN, which induces a more than 2 times higher degradation rate than bulk g-C3N4. This work offers a prospective route for template-free designing porous functional materials with improved properties and efficiently treating emerging pollutants such as 6PPD-Q, pathogenic bacteria, and antibiotic residues.